Mn2C MXene functionalized by oxygen is a semiconducting antiferromagnet and an efficient visible light absorber.

Abstract

Manganese-based MXenes are promising two-dimensional materials due to the broad palette of their magnetic phases and the possibility of experimental preparation because the corresponding MAX phase was already prepared. Here, we systematically investigated geometrical conformers and spin solutions of oxygen-terminated Mn2C MXene and performed subsequent many-body calculations to obtain reliable electronic and optical properties. Allowing energy-lowering using the correct spin ordering via supercell magnetic motifs is essential for the Mn2CO2 system. The stable ground-state Mn2CO2 conformation is antiferromagnetic (AFM) with zigzag lines of up and down spins on Mn atoms. The AFM nature is consistent with the parent MAX phase and even the clean depleted Mn2C sheet. Other magnetic states and geometrical conformations are energetically very close, providing state-switching possibilities in the material. Subsequent many-body GW and Bethe-Salpeter equation (BSE) calculations provide indirect semiconductor characteristics of AFM Mn2CO2 with a fundamental gap of 2.1 eV (and a direct gap of 2.4 eV), the first bright optical transition at 1.3 eV and extremely strongly bound (1.1 eV) first bright exciton. Mn2CO2 absorbs efficiently the whole visible light range and near ultraviolet range (between 10 and 20%).